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DOI: 10.1002/aenm.201200166
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decreased to 159 and 143 mAh/g for the ALD20 and ALD50
electrodes, respectively, with no decrease in reversible capacities. Correspondingly, the initial coulombic efficiencies respectively increased to 62.5% and 60.6% for the ALD20 and ALD50
electrodes. The increased efficiency can be attributed to the fact
that the Al2O3 layer mitigates the formation of SEI on the electrode surface through the reductive decomposition of electrolytes during initial discharge.
Figure 4a, b, and c show the dischargecharge curves of
untreated and Al2O3-coated electrodes at different current
rates. All cells were successively discharged and charged with
increasing current rates from 0.05 C to 2 C for five cycles at
each rate. It is found that the Al2O3-coating is also effective in
improving rate capability (see Figure 4 and S6). For the ALD20
electrode, 91.1%, 86.2%, 64.9%, and 52.8% of the capacity at
0.05 C were still accessible at current rates of 0.1, 0.2, 1, and 2 C,
respectively. In the case of the ALD50 electrode, 91.3%, 87.3%,
67.2%, and 57.0% of the capacity at 0.05 C were achieved, compared with capacity retentions of 87.9%, 80.2%, 52.4%, and
31.5% for the untreated electrode. Moreover, cycling at high
current density does not permanently damage the structure of
the electrode, given that the capacity is restored when the rate is
reduced to a low current rate (0.1 C). As it is well known, Al2O3 is
an insulated coating layer, however, this characteristic is not contradictory to the enhanced rate performance, because the Al2O3
coating layer can reduce the formation of SEI layer on electrode
surface, which results in large impedance; and the Al2O3 coating
layer is also beneficial to the structure maintenance of the electrode. Finally, the cycling performance is also improved after
Al2O3 coating of the electrode (Figure 4d). The untreated electrode presented an initial charge capacity of 258 mAh/g, which
slowly faded to 192 mAh/g after 50 cycles, with a capacity retention of 74.4%. The ALD20 and ALD50 electrodes exhibited initial
charge capacities of 282 and 255 mAh/g, which decayed to 225
and 211 mAh/g, with capacity retentions of 79.8% and 82.7%,
respectively. A thin layer of Al2O3 coating through the ALD technique on the electrode surface has been shown to effectively
improve the performance of inorganic electrodes. This is the
first example to demonstrate the effectiveness of this technique
in enhancing the performance of an organic electrode.
In conclusion, Na2C8H4O4 is firstly introduced as a novel
anode material for low-cost rechargeable room-temperature
Na-ion batteries. The material exhibits low Na insertion voltage
at 0.29 V. The Na2C8H4O4/KB composite electrode shows a
reversible capacity of 250 mAh/g, corresponding to a twoelectron transfer, with excellent cycling performance. By performing ALD Al2O3 coating on the surface of the Na2C8H4O4/
KB electrode, Na storage performance is significantly improved
in terms of initial coulombic efficiency, rate capability, and
cycling performance. Future work on the further reduction of
the irreversible capacity during the initial chargedischarge
process and on exploring Na storage mechanism is currently
in progress.
Experimental Section
Na2C8H4O4 was purchased from Alfa Aesar Company and used without
further treatment. Na2C8H4O4 and Ketjen black (EC-600JD, Ketjenblack
International, Japan) (80:20) were ball-milled in a planetary ball mill
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Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was supported by the National High Technology Research
and Development Program of China (Grant No. 2009AA033101), the
National Basic Research Program of China (Grant No. 2009CB220104),
the National Natural Science Foundation of China (Grant No.50972164),
Chinese Academy of Sciences Project (Grant No. KJCX2-YW-W26), and
the Hundred-Talent Project of the Chinese Academy of Sciences.
Received: March 9, 2012
Published online: May 11, 2012
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